Accurately metal-modulated bimetallic metal-organic frameworks as advanced trifunctional electrocatalysts

To fabricate efficient multifunctional electrocatalysts for energy storage and conversion is still a great challenge, due to the difficulty in precisely identifying and regulating catalytic active sites. Herein, a series of isostructural metal-organic frameworks (MOFs) with V-shaped trinuclear clust...

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Published inJournal of materials chemistry. A, Materials for energy and sustainability Vol. 9; no. 26; pp. 14682 - 1469
Main Authors Chen, Xin, Shao, Bing, Tang, Meng-Juan, He, Xing-Lu, Yang, Fu-Jie, Guo, Ze-Ping, Zhang, Zhong, He, Chun-Ting, Huang, Fu-Ping, Huang, Jin
Format Journal Article
LanguageEnglish
Published Cambridge Royal Society of Chemistry 06.07.2021
Subjects
active sites
Bimetals
Catalysts
catalytic activity
Chemical reduction
Coordination
Crystallography
Electrocatalysts
electrochemistry
energy
Energy storage
Hydrogen evolution reactions
hydrogen production
Metal clusters
Metal-organic frameworks
Metals
Mossbauer spectroscopy
Oxygen
Oxygen evolution reactions
oxygen production
Oxygen reduction reactions
Single crystals
spectroscopy
X-ray diffraction
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Abstract To fabricate efficient multifunctional electrocatalysts for energy storage and conversion is still a great challenge, due to the difficulty in precisely identifying and regulating catalytic active sites. Herein, a series of isostructural metal-organic frameworks (MOFs) with V-shaped trinuclear clusters was used as an ideal model to investigate the activity of trifunctional electrocatalysis for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and oxygen reduction reaction (ORR), as these clusters contain both coordination unsaturated metal sites (also known as open metal sites, OMSs) and coordination saturation metal sites (CSMSs), corresponding to both ends and the middle of the V-shaped cluster, respectively. Using a combination of single-crystal X-ray diffractometry, Mössbauer spectroscopy and theoretical calculations, the accurate metal sequence of trinuclear clusters and the regulation effect of the active sites were identified, revealing that the adjacent inactive site plays a significant role in regulating the catalytic performance of the endmost active site. The proposed model of metal cluster-based electrocatalysts facilitates the investigation on efficient multifunctional electrocatalysts as well as the related catalytic mechanisms. The atomic-level metal-modulated MOFs as an advanced trifunctional electrocatalyst for oxygen evolution reaction, hydrogen evolution reaction and oxygen reduction reaction.
AbstractList To fabricate efficient multifunctional electrocatalysts for energy storage and conversion is still a great challenge, due to the difficulty in precisely identifying and regulating catalytic active sites. Herein, a series of isostructural metal–organic frameworks (MOFs) with V-shaped trinuclear clusters was used as an ideal model to investigate the activity of trifunctional electrocatalysis for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and oxygen reduction reaction (ORR), as these clusters contain both coordination unsaturated metal sites (also known as open metal sites, OMSs) and coordination saturation metal sites (CSMSs), corresponding to both ends and the middle of the V-shaped cluster, respectively. Using a combination of single-crystal X-ray diffractometry, Mössbauer spectroscopy and theoretical calculations, the accurate metal sequence of trinuclear clusters and the regulation effect of the active sites were identified, revealing that the adjacent inactive site plays a significant role in regulating the catalytic performance of the endmost active site. The proposed model of metal cluster-based electrocatalysts facilitates the investigation on efficient multifunctional electrocatalysts as well as the related catalytic mechanisms.
To fabricate efficient multifunctional electrocatalysts for energy storage and conversion is still a great challenge, due to the difficulty in precisely identifying and regulating catalytic active sites. Herein, a series of isostructural metal-organic frameworks (MOFs) with V-shaped trinuclear clusters was used as an ideal model to investigate the activity of trifunctional electrocatalysis for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and oxygen reduction reaction (ORR), as these clusters contain both coordination unsaturated metal sites (also known as open metal sites, OMSs) and coordination saturation metal sites (CSMSs), corresponding to both ends and the middle of the V-shaped cluster, respectively. Using a combination of single-crystal X-ray diffractometry, Mössbauer spectroscopy and theoretical calculations, the accurate metal sequence of trinuclear clusters and the regulation effect of the active sites were identified, revealing that the adjacent inactive site plays a significant role in regulating the catalytic performance of the endmost active site. The proposed model of metal cluster-based electrocatalysts facilitates the investigation on efficient multifunctional electrocatalysts as well as the related catalytic mechanisms. The atomic-level metal-modulated MOFs as an advanced trifunctional electrocatalyst for oxygen evolution reaction, hydrogen evolution reaction and oxygen reduction reaction.
Author Chen, Xin
Huang, Jin
He, Xing-Lu
Huang, Fu-Ping
Zhang, Zhong
Guo, Ze-Ping
Yang, Fu-Jie
He, Chun-Ting
Shao, Bing
Tang, Meng-Juan
AuthorAffiliation Ministry of Education
Zhongkai University of Agriculture and Engineering
School of Physical Science and Technology
Guangxi Normal University
Key Laboratory of Functional Small Organic Molecule
College of Chemistry and Chemical Engineering
School of Chemistry and Pharmaceutical Sciences
Jiangxi Normal University
AuthorAffiliation_xml – name: School of Physical Science and Technology
– name: Guangxi Normal University
– name: Ministry of Education
– name: College of Chemistry and Chemical Engineering
– name: Key Laboratory of Functional Small Organic Molecule
– name: Zhongkai University of Agriculture and Engineering
– name: School of Chemistry and Pharmaceutical Sciences
– name: Jiangxi Normal University
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Electronic supplementary information (ESI) available: The syntheses and characterization of the catalyst, supplementary figures and tables. CCDC
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Snippet To fabricate efficient multifunctional electrocatalysts for energy storage and conversion is still a great challenge, due to the difficulty in precisely...
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SubjectTerms active sites
Bimetals
Catalysts
catalytic activity
Chemical reduction
Coordination
Crystallography
Electrocatalysts
electrochemistry
energy
Energy storage
Hydrogen evolution reactions
hydrogen production
Metal clusters
Metal-organic frameworks
Metals
Mossbauer spectroscopy
Oxygen
Oxygen evolution reactions
oxygen production
Oxygen reduction reactions
Single crystals
spectroscopy
X-ray diffraction
Title Accurately metal-modulated bimetallic metal-organic frameworks as advanced trifunctional electrocatalysts
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